注册 English

K、Mn助剂协同效应对Fe基催化剂上CO加氢制低碳烯烃反应性能的影响

陈嘉宁 ,  刘永梅

downloadPDF
引用本文: 陈嘉宁, 刘永梅. K、Mn助剂协同效应对Fe基催化剂上CO加氢制低碳烯烃反应性能的影响[J]. 燃料化学学报, 2013, 41(12): 1488-1494. shu
Citation:  CHEN Jia-ning, LIU Yong-mei. Effects of Mn-K synergistic action on iron-based catalyst for CO hydrogenation to light olefins[J]. Journal of Fuel Chemistry and Technology, 2013, 41(12): 1488-1494. shu

K、Mn助剂协同效应对Fe基催化剂上CO加氢制低碳烯烃反应性能的影响

    通讯作者: 刘永梅（1973- ），女，山西太原人，博士，副教授，主要从事分子筛合成及应用，E-mail：l_y_m@126.com。
  • 基金项目:

    国家自然科学基金（21076222）。 

摘要: 采用典型方法制备了不同Fe、Mn、K比例的铁基催化剂，利用X射线粉末衍射、N2吸附/脱附、扫描电镜、拉曼光谱、H2-TPR等手段对催化剂进行了表征，并考察了催化剂对CO加氢制低碳烯烃反应的催化性能。结果表明，Mn能有效促进活性相分散，抑制碳链增长，但Fe-Mn强相互作用不能有效增加低碳烃烯/烷比，α-Fe2O3作为活性铁物种前驱体对烯烃生成反应更加有利。K通过减少Mn以氧化物形式出现，增加FeMn化合物晶格缺陷，从而最终使Fe-Mn-K催化剂低碳烯烃收率显著高于Fe-Mn和Fe-K体系。

English

  • 

    1. [1] 王野, 成康, 张庆红. 一氧化碳加氢制碳氢化合物反应选择性的调控[J]. 中国科学: 化学, 2012, 42(4): 363-375. (WANG Ye, CHENG Kang, ZHANG Qing-hong. Selectivity tuning for the hydrogenation of carbon monoxide into hydrocarbons[J]. Scientia Sinica Chimica, 2012, 42(4): 363-375.)[1] 王野, 成康, 张庆红. 一氧化碳加氢制碳氢化合物反应选择性的调控[J]. 中国科学: 化学, 2012, 42(4): 363-375. (WANG Ye, CHENG Kang, ZHANG Qing-hong. Selectivity tuning for the hydrogenation of carbon monoxide into hydrocarbons[J]. Scientia Sinica Chimica, 2012, 42(4): 363-375.)

    2. [2] 胡浩, 叶丽萍, 应卫勇, 房鼎业. 国外甲醇制烯烃生产工艺与反应器开发现状[J]. 现代化工, 2008, 28(1): 82-86. (HU hao, YE Li-ping, YING Wei-yong, FANG Ding-ye. Advancement on methanol-to-olefin process technology and reactor design overseas[J]. Modern Chemical Industry, 2008, 28(1): 82-86.)[2] 胡浩, 叶丽萍, 应卫勇, 房鼎业. 国外甲醇制烯烃生产工艺与反应器开发现状[J]. 现代化工, 2008, 28(1): 82-86. (HU hao, YE Li-ping, YING Wei-yong, FANG Ding-ye. Advancement on methanol-to-olefin process technology and reactor design overseas[J]. Modern Chemical Industry, 2008, 28(1): 82-86.)

    3. [3] FRANCESCA L B, SACHIN C, UNNI O, MARILYNE B, FABIEN O, BENOIT L. Conversion of methanol into light olefins over ZSM-5 zeolite: Strategy to enhance propene selectivity[J]. App Catal A: Gen, 2012, 447: 178-185.[3] FRANCESCA L B, SACHIN C, UNNI O, MARILYNE B, FABIEN O, BENOIT L. Conversion of methanol into light olefins over ZSM-5 zeolite: Strategy to enhance propene selectivity[J]. App Catal A: Gen, 2012, 447: 178-185.

    4. [4] ZHANG Q H, KANG J C, WANG Y. Development of novel catalysts for Fischer-Tropsch synthesis: Tuning the product selectivity[J]. Chem Cat Chem, 2010, 2(9): 1030-1058.[4] ZHANG Q H, KANG J C, WANG Y. Development of novel catalysts for Fischer-Tropsch synthesis: Tuning the product selectivity[J]. Chem Cat Chem, 2010, 2(9): 1030-1058.

    5. [5] JENSEN K B, MASSOTH F E. Studies on iron-manganese oxide carbon monoxide catalysts: I. Structure of reduced catalyst[J]. J Catal, 1985, 92(1): 98-108.[5] JENSEN K B, MASSOTH F E. Studies on iron-manganese oxide carbon monoxide catalysts: I. Structure of reduced catalyst[J]. J Catal, 1985, 92(1): 98-108.

    6. [6] MALESSA R, BAERNS M. Iron/manganese oxide catalysts for Fischer-Tropsch synthesis. 4. Activity and selectivity[J].Ind Eng Chem Res, 1988, 27(2): 279-283.[6] MALESSA R, BAERNS M. Iron/manganese oxide catalysts for Fischer-Tropsch synthesis. 4. Activity and selectivity[J].Ind Eng Chem Res, 1988, 27(2): 279-283.

    7. [7] LEITH I R, HOWDEN M G. Temperature-programmed reduction of mixed iron-manganese oxide catalysts in hydrogen and carbon monoxide[J].Appl Catal, 1988, 37: 75-92.[7] LEITH I R, HOWDEN M G. Temperature-programmed reduction of mixed iron-manganese oxide catalysts in hydrogen and carbon monoxide[J].Appl Catal, 1988, 37: 75-92.

    8. [8] ERIKSSON S, NYLEN U, ROJAS S, BOUTONNET M. Preparation of catalysts from microemulsions and their applications in heterogeneous catalysis[J]. Appl Catal A: Gen, 2004, 265(2): 207-219.[8] ERIKSSON S, NYLEN U, ROJAS S, BOUTONNET M. Preparation of catalysts from microemulsions and their applications in heterogeneous catalysis[J]. Appl Catal A: Gen, 2004, 265(2): 207-219.

    9. [9] DAS C K, DAS N S, CHOUDHURY D P, RAVICHANDRAN G, CHAKRABARTY D K. Hydrogenation of carbon monoxide on unsupported Fe-Mn-K catalysts for the synthesis of lower alkenes: Promoter effect of manganese[J]. Appl Catal A: Gen, 1994, 111(2): 119-132.[9] DAS C K, DAS N S, CHOUDHURY D P, RAVICHANDRAN G, CHAKRABARTY D K. Hydrogenation of carbon monoxide on unsupported Fe-Mn-K catalysts for the synthesis of lower alkenes: Promoter effect of manganese[J]. Appl Catal A: Gen, 1994, 111(2): 119-132.

    10. [10] WANG C, WANG Q, SUN X, XU L. CO hydrogenation to light alkenes over Mn/Fe catalysts prepared by coprecipitation and sol-gel methods[J].Catal Lett, 2005, 105(1): 93-101.[10] WANG C, WANG Q, SUN X, XU L. CO hydrogenation to light alkenes over Mn/Fe catalysts prepared by coprecipitation and sol-gel methods[J].Catal Lett, 2005, 105(1): 93-101.

    11. [11] HUO C F, WU B S, GAO P, YANG Y, LI Y W, JIAO H J. The mechanism of potassium promoter: Enhancing the stability of active surfaces[J].Angew Chem Int Ed, 2011, 50(32): 7403-7406.[11] HUO C F, WU B S, GAO P, YANG Y, LI Y W, JIAO H J. The mechanism of potassium promoter: Enhancing the stability of active surfaces[J].Angew Chem Int Ed, 2011, 50(32): 7403-7406.

    12. [12] DE SMIT E, WECKHUYSEN B M. The renaissance of iron-based Fischer-Tropsch synthesis: On the multifaceted catalyst deactivation behaviour[J]. Chem Soc Rev, 2008, 37(12): 2758-2781.[12] DE SMIT E, WECKHUYSEN B M. The renaissance of iron-based Fischer-Tropsch synthesis: On the multifaceted catalyst deactivation behaviour[J]. Chem Soc Rev, 2008, 37(12): 2758-2781.

    13. [13] YANG L X, ZHU Y J, TONG H, WANG W W, CHENG G F. Low temperature synthesis of Mn3O4 polyhedral nanocrystals and magnetic study[J]. J Solid State Chem, 2006, 179(4): 1225-1229.[13] YANG L X, ZHU Y J, TONG H, WANG W W, CHENG G F. Low temperature synthesis of Mn3O4 polyhedral nanocrystals and magnetic study[J]. J Solid State Chem, 2006, 179(4): 1225-1229.

    14. [14] 郭荷芹, 李德宝, 陈从标, 范志宏, 孙予罕. V2O5/CeO2催化剂上甲醇氧化一步法合成二甲氧基甲烷[J]. 催化学报, 2012, 33(5): 813-818. (GUO He-qin, LI De-bao, CHEN Cong-biao, FAN Zhi-hong, SUN Yu-han. One-step oxidation of methanol to dimethoxymethane on V2O5/CeO2 catalyst[J]. Chinese Journal of Catalysis, 2012, 33(5): 813-813.)[14] 郭荷芹, 李德宝, 陈从标, 范志宏, 孙予罕. V2O5/CeO2催化剂上甲醇氧化一步法合成二甲氧基甲烷[J]. 催化学报, 2012, 33(5): 813-818. (GUO He-qin, LI De-bao, CHEN Cong-biao, FAN Zhi-hong, SUN Yu-han. One-step oxidation of methanol to dimethoxymethane on V2O5/CeO2 catalyst[J]. Chinese Journal of Catalysis, 2012, 33(5): 813-813.)

    15. [15] De FARIA D L A, SILVA SV, De OLIVEIRA M T. Raman microspectroscopy of some iron oxides and oxyhydroxides[J].J Raman Spectrosc, 1997, 28(11): 873-878.[15] De FARIA D L A, SILVA SV, De OLIVEIRA M T. Raman microspectroscopy of some iron oxides and oxyhydroxides[J].J Raman Spectrosc, 1997, 28(11): 873-878.

    16. [16] DUBAL D P, DHAWALE D S, SALUNKHE R R, LOKHANDE C D. Conversion of interlocked cube-like Mn3O4 into nanoflakes of layered birnessite MnO2 during supercapacitive studies[J]. J Alloy Compd, 2010, 496(2): 370-375.[16] DUBAL D P, DHAWALE D S, SALUNKHE R R, LOKHANDE C D. Conversion of interlocked cube-like Mn3O4 into nanoflakes of layered birnessite MnO2 during supercapacitive studies[J]. J Alloy Compd, 2010, 496(2): 370-375.

    17. [17] SANKAR K V, SENTHILKUMAR S T, BERCHMANS L J, SANJEEVIRAJA C, SELVAN R K. Effect of reaction time on the synthesis and electrochemical properties of Mn3O4 nanoparticles by microwave assisted reflux method[J]. Appl Surf Sci, 2012, 259: 624-630.[17] SANKAR K V, SENTHILKUMAR S T, BERCHMANS L J, SANJEEVIRAJA C, SELVAN R K. Effect of reaction time on the synthesis and electrochemical properties of Mn3O4 nanoparticles by microwave assisted reflux method[J]. Appl Surf Sci, 2012, 259: 624-630.

    18. [18] YANG Y, XIANG H W, XU Y Y, BAI L, LI Y Y. Effect of potassium promoter on precipitated iron-manganese catalyst for Fischer-Tropsch synthesis[J]. Appl Catal A: Gen, 2004, 266(2): 181-194.[18] YANG Y, XIANG H W, XU Y Y, BAI L, LI Y Y. Effect of potassium promoter on precipitated iron-manganese catalyst for Fischer-Tropsch synthesis[J]. Appl Catal A: Gen, 2004, 266(2): 181-194.

    19. [19] GAUBE J, KLEIN H F. The promoter effect of alkali in Fischer-Tropsch iron and cobalt catalysts[J]. Appl Catal A: Gen, 2008, 350(1): 126-132.[19] GAUBE J, KLEIN H F. The promoter effect of alkali in Fischer-Tropsch iron and cobalt catalysts[J]. Appl Catal A: Gen, 2008, 350(1): 126-132.

    20. [20] LEITH I R, HOWDEN M G. Temperature-programmed reduction of mixed iron-manganese oxide catalysts in hydrogen and carbon monoxide[J].Appl Catal, 1988, 37: 75-92.[20] LEITH I R, HOWDEN M G. Temperature-programmed reduction of mixed iron-manganese oxide catalysts in hydrogen and carbon monoxide[J].Appl Catal, 1988, 37: 75-92.

    21. [21] VENTER J, KAMINSKY M, GEOFFROY G L, ALBERT VANNICE M. Carbon-supported Fe-Mn and K-Fe-Mn clusters for the synthesis of C2~C4 olefins from CO and H2: I. Chemisorption and catalytic behavior[J]. J Catal, 1987, 103(2): 450-465.[21] VENTER J, KAMINSKY M, GEOFFROY G L, ALBERT VANNICE M. Carbon-supported Fe-Mn and K-Fe-Mn clusters for the synthesis of C2~C4 olefins from CO and H2: I. Chemisorption and catalytic behavior[J]. J Catal, 1987, 103(2): 450-465.

    22. [22] JENSEN K B, MASSOTH F E. Studies on iron-manganese oxide carbon monoxide catalysts: I. Structure of reduced catalyst[J]. J Catal, 1985, 92(1): 98-108.[22] JENSEN K B, MASSOTH F E. Studies on iron-manganese oxide carbon monoxide catalysts: I. Structure of reduced catalyst[J]. J Catal, 1985, 92(1): 98-108.

    23. [23] DE SMIT E, WECKHUYSEN B M. The renaissance of iron-based Fischer-Tropsch synthesis: On the multifaceted catalyst deactivation behaviour[J]. Chem Soc Rev, 2008, 37(12): 2758-2781.[23] DE SMIT E, WECKHUYSEN B M. The renaissance of iron-based Fischer-Tropsch synthesis: On the multifaceted catalyst deactivation behaviour[J]. Chem Soc Rev, 2008, 37(12): 2758-2781.

    24. [24] BUKUR D B, MUKESH D S, PATAL A. Promoter effects on precipitated iron catalysts for Fischer-Tropsch synthesis[J].Ind Eng Chem Res, 1990, 29(2): 194-204.[24] BUKUR D B, MUKESH D S, PATAL A. Promoter effects on precipitated iron catalysts for Fischer-Tropsch synthesis[J].Ind Eng Chem Res, 1990, 29(2): 194-204.

    25. [25] YANG C, ZHAO H, HOU Y, MA D. Fe5C2 nanoparticles: A facile bromide-induced synthesis and as an active phase for Fischer-Tropsch synthesis[J]. J Am Chem Soc, 2012, 134(38): 15814-15821.[25] YANG C, ZHAO H, HOU Y, MA D. Fe5C2 nanoparticles: A facile bromide-induced synthesis and as an active phase for Fischer-Tropsch synthesis[J]. J Am Chem Soc, 2012, 134(38): 15814-15821.

  • 加载中
WeChat 扫一扫看文章
计量
  • PDF下载量:  0
  • 文章访问数:  801
  • HTML全文浏览量:  80
文章相关
  • 收稿日期:  2013-07-15
  • 网络出版日期:  2013-10-12
通讯作者: 陈斌, bchen63@163.com
  • 1. 

    沈阳化工大学材料科学与工程学院 沈阳 110142

  1. 本站搜索
  2. 百度学术搜索
  3. 万方数据库搜索
  4. CNKI搜索

/

返回文章

All Rights Reserved by the Chinese Chemical Society   中国化学会 版权所有 京ICP备05002797号

本系统由北京仁和汇智信息技术有限公司开发    技术支持: info@rhhz.net